Cross was born in Douai on May 20, 1856 and grew up in Lille. He studied at the École des Beaux-Arts. His early works, portraits and still lifes, were in the dark colors of realism, but after meeting with Claude Monet in 1883, he painted in the brighter colors of Impressionism. In 1884, Cross cofounded the Société des Artistes Indépendants. He went on to become one of the principal exponents of Neo-Impressionism. He began his Pointillist period after spending time with Paul Signac in 1904. His later works are Fauvist, perhaps influenced by his acquaintance with Henri Matisse.
His final years, plagued by rheumatism, were spent in Saint-Clair, where he died May 16, 1910.